The applications of polycrystalline films range from interconnects in the electronics and semiconductor industry to solar cells and as corrosion protection. Despite their significance, factors that determine their microstructure and morphology remain largely unsolved. The surface and microstructure of electrodeposited polycrystalline Cu films were investigated. This involves looking at the later growth stages of Cu films using different surface and bulk characterization techniques. The surface evolution of an electrodeposited Cu film was imaged in real-time using a Highspeed Atomic Force Microscope (HS-AFM). This provides details about how the film structure coarsens with time. The high-resolution video showed accelerated local grain growth and grain overgrowth at different locations of the film. A combination of both of these mechanisms could drive structural coarsening. The microstructure could play a role in inducing faster growth in certain grains. How the local and large-scale roughness varies with film thickness is studied by scaling analysis. As a complement to scaling analysis, variation in the local slope with thickness is calculated using slope analysis. Rapid growth was observed in the regions where the HS-AFM tip was scanning. The removal of oxygen adlayer from the surface by the tip could promote faster growth in these regions. Pulsed electrodeposition produced Cu films with hexagonal structures. They are known to be twinned which is a desirable feature in applications that require superior mechanical and electrical properties. The effect of electrode potential on grain size was studied. Using a watershed segmentation algorithm, the grain area was calculated from the AFM images. The grain area showed an increasing trend with increasing overpotential. Slope analysis on the ’hexagons’ and the complete films electrodeposited at higher potential revealed higher slopes and distinct slope distribution. Cross-sectional Focused Ion Beam (FIB) milling confirmed that horizontal twins are present in the pulse-deposited Cu films. The hexagonal pyramids with twins could be produced by one of the two mechanisms, stress relaxation during the ’OFF’ period of pulsing or driven by screw dislocation. We attribute the origin of the hexagons to spiralling screw dislocations. A template matching algorithm was developed to try and correlate the surface and microstructural data of a Cu film grown on a microelectrode. It involved matching the AFM and Electron Back Scatter Diffraction (EBSD) data on the later FIB milled sample, thus relating surface topography to crystallographic orientation. The crystallographic orientation of the edge of the microelectrode and its centre showed different orientations, switching from (111) to (110). Twinning was investigated at the edge and the centre of the microelectrode revealing the presence of stacking fault twins in both of these regions
